A highly anisotropic toughness behavior has been revealed on a forged AA6061 aluminum alloy by toughness tests with CT specimens. e toughness values with specimens loaded on the longitudinal direction are larger than that loaded on the transverse direction due to the anisotropic shape and distribution of coarse precipitates induced by the morphological anisotropy of grains during forging process. Synchrotron radiation computed tomography analysis on as-received material and arrested cracks revealed different fracture modes for the two loading configurations. e damage mechanism has been validated by finite element simulations based on the Gurson-Tvergaard-Needleman micromechanical damage model with different sets of damage parameters for the two loading configurations obtained from quantitative void volume fraction analysis on SRCT data, in situ SEM experiments, and SRCT microstructural analysis.